无机汞和甲基汞在l-半胱氨酸覆盖的CdSe纳米粒子存在下的转化

Xian-Yang Shi, Jingchan Zhao, Yongchen Wang, R. Mason
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引用次数: 1

摘要

水环境中汞(Hg)形态的转化是汞的命运、运输和甲基汞(CH3Hg;甲基汞),这是引起大多数人类健康问题的形式。汞在表面形态之间的转化尚未得到充分的研究,但在这里,我们报告了无机汞(HgII)和甲基汞与硫系纳米颗粒(NPs)的相互作用;特别是l -半胱氨酸覆盖的CdSe纳米晶体。本研究通过考察产物组成、反应质量平衡和液固两相分布,揭示了汞的形态转化及其相互作用机制。结果表明,HgII对CdSe NPs光致发光的猝灭作用大于MeHg,即使在nM范围内,HgII也能引起明显的猝灭作用。在实验溶液中,超过90%的HgII存在于固相,而大多数MeHg存在于液相。无二甲基汞((CH3)2Hg;二甲基汞(DMeHg)是由甲基汞与NPs相互作用产生的,与微粒的发现相反。然而,当MeHg + NPs混合物暴露在光线下时,MeHg迅速而完全地转化为HgII。提出了一种MeHg降解方案,并得出了HgSe的沉淀加速了MeHg降解的结论。这些结果为在NPs存在的情况下环境水体中甲基汞降解的非生物途径提供了见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
The Transformation of Inorganic and Methylmercury in the Presence of l-Cysteine Capped CdSe Nanoparticles
Transformations of mercury (Hg) forms in the aquatic environment is a crucial aspect of Hg fate, transport and the bioaccumulation of methylmercury (CH3Hg; MeHg), which is the form that drives most human health concerns. Transformations between Hg forms on surfaces have been inadequately studied but here we report on the interaction of inorganic Hg (HgII) and MeHg with chalcogenide nanoparticles (NPs); specifically L-cysteine capped CdSe nanocrystals. The study sheds light on the transformation of the Hg species and the interaction mechanisms, by examining the product composition, reaction mass balance and the distribution between the liquid and solid phase. The results showed that the quenching of the photoluminescence (PL) of CdSe NPs was greater for HgII than MeHg, and that HgII caused significant PL quenching even when its concentration was in the nM range. Over 90% of HgII was found associated with the solid phase while most MeHg existed in the liquid phase in the experimental solutions. No dimethylmercury ((CH3)2Hg; DMeHg) was produced from the interaction of MeHg and the NPs, in contrast to findings with microparticles. However, a fast and complete MeHg transformation into HgII occurred when the MeHg + NPs mixture was exposed to light. A scheme for the MeHg degradation was derived and is presented, and it was concluded that the precipitation of HgSe accelerated the MeHg degradation. These results provide insight into the abiotic pathways for MeHg degradation in environmental waters in the presence of NPs.
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